Detailed Insight into the CZTS/CdS Interface Modification by Air Annealing in Monograin Layer Solar Cells

Abstract

Relatively fast achievements in the kesterite solar cell technology have been made over the last decade, but the experimental efficiency is still ∼13%. One proposed reason is an inappropriate band alignment with Cu2ZnSnS4 (CZTS) and CdS that results in strong interface recombination losses. Results of this work show that the temperature and duration of air annealing of the CZTS/CdS heterojunction are essential for device performance. Soft annealing slightly improved the device efficiency due to the elemental intermixing at the interface. On the other hand, extended annealing increased absorber band gap energy, resulting in higher VOC values, indicating the improved Cu–Zn ordering in the CZTS structure, which also could be expected to have a beneficial influence on the device performance. However, interface analysis revealed that the CZTS absorber surface layer was Cu-rich, providing the reason for the reduction in CZTS solar cell performance. The effect of annealing on the interface defects was analyzed by the capacitance–frequency–voltage (C–V–f) analysis combined with SCAPS simulations. C–V–f-based loss maps showed that air annealing modifies the density distribution of asymmetrical interface states at the CZTS/CdS interface, which becomes fully symmetrical for longer annealing times at 200 °C.